Organic-inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light-emitting diodes, lasers, and light-emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light-emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A(-1) have been achieved. Although perovskite light-emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light-emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower-dimensionality layered and three-dimensional perovskites, nanostructures, charge-transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light-emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light-emitting devices.
Multiphoton absorption processes enable many technologically important applications, such as in vivo imaging, photodynamic therapy and optical limiting, and so on. Specifically, higher-order nonlinear absorption such as five-photon absorption offers significant advantages of greater spatial confinement, increased penetration depth, reduced autofluorescence, enhanced sensitivity and improved resolution over lower orders in bioimaging. Organic chromophores and conventional semiconductor nanocrystals are leaders in two-/three-photon absorption applications, but face considerable challenges from their small five-photon action cross-sections. Herein, we reveal that the family of halide perovskite colloidal nanocrystals transcend these constraints with highly efficient five-photon-excited upconversion fluorescence—unprecedented for semiconductor nanocrystals. Amazingly, their multidimensional type I (both conduction and valence band edges of core lie within bandgap of shell) core–shell (three-dimensional methylammonium lead bromide/two-dimensional octylammonium lead bromide) perovskite nanocrystals exhibit five-photon action cross-sections that are at least 9 orders larger than state-of-the-art specially designed organic molecules. Importantly, this family of halide perovskite nanocrystals may enable fresh approaches for next-generation multiphoton imaging applications.
The unique mesoscopic perovskite film architecture of 2D microplatelets on top of 3D nanocrystals enable an energy cascade, yielding highly efficient light-emitting diodes.
Multiple exciton generation (MEG) or carrier multiplication, a process that spawns two or more electron–hole pairs from an absorbed high-energy photon (larger than two times bandgap energy Eg), is a promising way to augment the photocurrent and overcome the Shockley–Queisser limit. Conventional semiconductor nanocrystals, the forerunners, face severe challenges from fast hot-carrier cooling. Perovskite nanocrystals possess an intrinsic phonon bottleneck that prolongs slow hot-carrier cooling, transcending these limitations. Herein, we demonstrate enhanced MEG with 2.25Eg threshold and 75% slope efficiency in intermediate-confined colloidal formamidinium lead iodide nanocrystals, surpassing those in strongly confined lead sulfide or lead selenide incumbents. Efficient MEG occurs via inverse Auger process within 90 fs, afforded by the slow cooling of energetic hot carriers. These nanocrystals circumvent the conundrum over enhanced Coulombic coupling and reduced density of states in strongly confined nanocrystals. These insights may lead to the realization of next generation of solar cells and efficient optoelectronic devices.
We report the high yield synthesis of about 11 nm sized CHNHPbBr nanocrystals with near-unity photoluminescence quantum yield. The nanocrystals are formed in the presence of surface-binding ligands through their direct precipitation in a benzyl alcohol/toluene phase. The benzyl alcohol plays a pivotal role in steering the surface ligands binding motifs on the NC surface, resulting in enhanced surface-trap passivation and near-unity PLQY values. We further demonstrate that thin films from purified CHNHPbBr nanocrystals are stable >4 months in air, exhibit high optical gain (about 520 cm), and display stable, ultralow amplified spontaneous emission thresholds of 13.9 ± 1.3 and 569.7 ± 6 μJ cm at one-photon (400 nm) and two-photon (800 nm) absorption, respectively. To the best of our knowledge, the latter signifies a 5-fold reduction of the lowest reported threshold value for halide perovskite nanocrystals to date, which makes them ideal candidates for light-emitting and low-threshold lasing applications.
The synthesis of all-inorganic cesium lead halide perovskite quantum dots (QDs) typically requires high temperatures, stringent conditions, large quantities of surface ligands, and judicious purification steps to overcome ligand-induced charge injection barriers in optoelectronic devices. Low-temperature syntheses generally require lower ligand concentrations, but are severely limited by the low solubility of the Cs precursor. We describe an innovative and general approach under ambient conditions to overcome these solubility limitations, by employing crown ethers. The crown ethers facilitate complete dissolution of the CsBr precursor, rendering CsPbBr3 QD inks practical for device fabrication. The resultant LEDs displayed bright green emission, with a current efficiency, and external quantum efficiency of 9.22 cd A -1 and 2.64%, respectively. This represents the first LED based on CsPbBr3 QDs prepared at room temperature. Lastly, the crown ethers form core-shell structures, opening new avenues to exploit their strong coordination strength.
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